<p>A key challenge in heterogeneous catalysis is to design atomically dispersed catalysts with high surface density, while simultaneously preventing agglomeration and promoting electronic metal-support interaction. Transition metal dichalcogenides (TMDs), such as platinum diselenide (PtSe<sub>2</sub>), offer a promising solution due to their unique structural and electronic properties. This study proposes a catalyst design that utilizes atomically dispersed transition metal species within the topmost layer of TMD as catalytic reaction sites. The substantial presence of surface-exposed Pt species on PtSe<sub>2</sub> and their role as catalytic reaction sites are elucidated using <i>operando</i> ambient-pressure X-ray photoelectron spectroscopy. Moreover, significantly high O<sub>2</sub> coverage on PtSe<sub>2</sub>, achieved by mitigating the exclusive adsorption of carbon monoxide (CO), leads to enhanced CO oxidation performance. The characteristic <i>d</i>-band structure and resulting high O<sub>2</sub> coverage of PtSe<sub>2</sub> are further confirmed with density functional theory calculations. Overall, this study highlights the potential of densely distributed atomic transition metal on TMDs, which allows electronic metal-chalcogen interactions and diverse reaction mechanisms.</p>

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Enhanced catalytic activity on atomically dispersed PtSe2 two-dimensional layers

  • Gyuho Han,
  • Hyuk Choi,
  • Jong Hun Kim,
  • Daeho Kim,
  • Sang Sub Han,
  • Hyewon Park,
  • Si Woo Lee,
  • Ki-jeong Kim,
  • Jeongjin Kim,
  • Min Gyu Kim,
  • Yeonwoong Jung,
  • Hyun You Kim,
  • Jeong Young Park

摘要

A key challenge in heterogeneous catalysis is to design atomically dispersed catalysts with high surface density, while simultaneously preventing agglomeration and promoting electronic metal-support interaction. Transition metal dichalcogenides (TMDs), such as platinum diselenide (PtSe2), offer a promising solution due to their unique structural and electronic properties. This study proposes a catalyst design that utilizes atomically dispersed transition metal species within the topmost layer of TMD as catalytic reaction sites. The substantial presence of surface-exposed Pt species on PtSe2 and their role as catalytic reaction sites are elucidated using operando ambient-pressure X-ray photoelectron spectroscopy. Moreover, significantly high O2 coverage on PtSe2, achieved by mitigating the exclusive adsorption of carbon monoxide (CO), leads to enhanced CO oxidation performance. The characteristic d-band structure and resulting high O2 coverage of PtSe2 are further confirmed with density functional theory calculations. Overall, this study highlights the potential of densely distributed atomic transition metal on TMDs, which allows electronic metal-chalcogen interactions and diverse reaction mechanisms.